Clarifying the Relationship between the Lithium Deposition Coverage and Microstructure in Lithium Metal Batteries

Journal Article (2022)
Author(s)

Qidi Wang (TU Delft - RST/Storage of Electrochemical Energy)

C. Zhao (TU Delft - RST/Storage of Electrochemical Energy)

Shuwei Wang (Tsinghua University)

Jianlin Wang (Chinese Academy of Sciences)

M. Liu (TU Delft - RST/Storage of Electrochemical Energy)

S Ganapathy (TU Delft - RID/TS/Instrumenten groep)

Xuedong Bai (Chinese Academy of Sciences)

Baohua Li (Tsinghua University)

Marnix Wagemaker (TU Delft - RST/Storage of Electrochemical Energy)

Research Group
RST/Storage of Electrochemical Energy
Copyright
© 2022 Q. Wang, C. Zhao, Shuwei Wang, Jianlin Wang, M. Liu, S. Ganapathy, Xuedong Bai, Baohua Li, M. Wagemaker
DOI related publication
https://doi.org/10.1021/jacs.2c08849
More Info
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Publication Year
2022
Language
English
Copyright
© 2022 Q. Wang, C. Zhao, Shuwei Wang, Jianlin Wang, M. Liu, S. Ganapathy, Xuedong Bai, Baohua Li, M. Wagemaker
Research Group
RST/Storage of Electrochemical Energy
Issue number
48
Volume number
144
Pages (from-to)
21961-21971
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Abstract

Improving the reversibility of lithium metal batteries is one of the challenges in current battery research. This requires better fundamental understanding of the evolution of the lithium deposition morphology, which is very complex due to the various parameters involved in different systems. Here, we clarify the fundamental origins of lithium deposition coverage in achieving highly reversible and compact lithium deposits, providing a comprehensive picture in the relationship between the lithium microstructure and solid electrolyte interphase (SEI) for lithium metal batteries. Systematic variation of the salt concentration offers a framework that brings forward the different aspects that play a role in cycling reversibility. Higher nucleation densities are formed in lower concentration electrolytes, which have the advantage of higher lithium deposition coverage; however, it goes along with the formation of an organic-rich instable SEI which is unfavorable for the reversibility during (dis)charging. On the other hand, the growth of large deposits benefiting from the formation of an inorganic-rich stable SEI is observed in higher concentration electrolytes, but the initial small nucleation density prevents full coverage of the current collector, thus compromising the plated lithium metal density. Taking advantages of the paradox, a nanostructured substrate is rationally applied, which increases the nucleation density realizing a higher deposition coverage and thus more compact plating at intermediate concentration (∼1.0 M) electrolytes, leading to extended reversible cycling of batteries.